Functional Carbonaceous Networks as Electrodes in Energy Storage Devices

电化学储能系统的发展在很大程度上取决于新型高性能电极材料的发展。在研究各种无机和有机电活性材料的同时，杂原子掺杂和/或功能化碳材料近年来因其在高性能电化学储能器件（包括锂离子电池和电化学电容器）中的巨大潜力而备受关注。然而，在先前报道的大多数情况下，基于现有的合成技术，杂原子和/或含氧官能团在母碳结构（如碳纳米管或石墨烯）中的浓度、分布和成键状态难以控制，这极大地限制了杂原子掺杂到碳材料中对其电化学性能影响的评估。另一方面，共轭高度交联的多孔聚合物网络可以高度定义官能团或杂原子的结合。然而，由于这些网络显示出低电导率，它们在电极上的使用相当有限。在本项目中，我们将通过合理合成和控制热解具有特定功能的共轭聚合物网络来制备功能碳质网络，并与其他导电材料如碳纳米管、石墨烯和纳米级金属集流器等构建其复合材料。这些新型材料和复合材料将被用作储能装置的电极，重点是了解这些碳基电极的结构-性能关系。结合对功能性碳质网络及其复合材料的化学功能、结构和界面对其电化学性能的影响的全面研究，该项目将使用优化的功能性碳质网络电极提供一类新的高性能不对称电化学电池。

The advancement of electrochemical energy storage systems highly depends on the development of novel high performance electrode materials. While a variety of inorganic and organic electroactive materials have been investigated, heteroatom-doped and/or functionalized carbon materials have recently attracted much attention because of their great potential in high performance electrochemical energy storage devices including lithium ion batteries and electrochemical capacitors. Yet, in most cases reported previously, the concentration, distribution, and bonding state of heteroatoms and/or oxygen-containing functional groups in the parent carbon structures (e.g., carbon nanotubes or graphene) are hardly controllable based on the existing synthetic techniques, which significantly limits the evaluation of the influence of heteroatoms doped into carbon materials on their electrochemical performance. Conjugated highly cross-linked porous polymer networks on the other hand enable a highly defined incorporation of functional groups or heteroatoms. However, their usage for electrodes is rather limited as these networks display low conductivities. In this project we will prepare functional carbonaceous networks by rational synthesis and controlled pyrolysis of conjugated polymer networks with specific functionalities, as well as construct their composites with other electrically conductive materials such as carbon nanotubes, graphene, and nanoscale metallic current collectors. These novel materials and composites will be exploited as electrodes in energy storage devices, with emphasis on the understanding of the structure-property relationship of these carbon-based electrodes. Combined with a comprehensive investigation of the effect of chemical functionalities, structure, and interfaces of functional carbonaceous networks and their composites on their electrochemical performance, the project will provide a new class of high performance asymmetric electrochemical cells using optimized functional carbonaceous network-based electrodes.